Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 132, Issue 5, Pages 1545-1557Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ja904906v
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Funding
- Chemical Sciences, Geosciences and Biosciences Division of the Office of Basic Energy Sciences, U.S. Department of Energy [DE-FG02-06ER15788, DE-SC0001011]
- UNC EFRC
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The mechanism of Ce(IV) water oxidation catalyzed by [Ru(tpy)(bpm)(OH2)](2+) (tpy = 2,2':6',2 ''-terpyridine; bpm = 2,2'-bipyrimidine) and related single-site catalysts has been determined by a combination of mixing and stopped-flow experiments with spectrophotometric monitoring. The mechanism features O---O coupling by water attack on Ru-V=O3+ and three peroxidic intermediates that have been characterized by a combination of spectroscopy and DFT calculations.
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